Cargando…

Charge Carriers Are Not Affected by the Relatively Slow-Rotating Methylammonium Cations in Lead Halide Perovskite Thin Films

[Image: see text] Recently, several studies have investigated dielectric properties as a possible origin of the exceptional optoelectronic properties of metal halide perovskites (MHPs). In this study we investigated the temperature-dependent dielectric behavior of different MHP films at different fr...

Descripción completa

Detalles Bibliográficos
Autores principales: Caselli, Valentina M., Fischer, Mathias, Meggiolaro, Daniele, Mosconi, Edoardo, De Angelis, Filippo, Stranks, Samuel D., Baumann, Andreas, Dyakonov, Vladimir, Hutter, Eline M., Savenije, Tom J.
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2019
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6734799/
https://www.ncbi.nlm.nih.gov/pubmed/31398042
http://dx.doi.org/10.1021/acs.jpclett.9b02160
_version_ 1783450222935932928
author Caselli, Valentina M.
Fischer, Mathias
Meggiolaro, Daniele
Mosconi, Edoardo
De Angelis, Filippo
Stranks, Samuel D.
Baumann, Andreas
Dyakonov, Vladimir
Hutter, Eline M.
Savenije, Tom J.
author_facet Caselli, Valentina M.
Fischer, Mathias
Meggiolaro, Daniele
Mosconi, Edoardo
De Angelis, Filippo
Stranks, Samuel D.
Baumann, Andreas
Dyakonov, Vladimir
Hutter, Eline M.
Savenije, Tom J.
author_sort Caselli, Valentina M.
collection PubMed
description [Image: see text] Recently, several studies have investigated dielectric properties as a possible origin of the exceptional optoelectronic properties of metal halide perovskites (MHPs). In this study we investigated the temperature-dependent dielectric behavior of different MHP films at different frequencies. In the gigahertz regime, dielectric losses in methylammonium-based samples are dominated by the rotational dynamics of the organic cation. Upon increasing the temperature from 160 to 300 K, the rotational relaxation time, τ, decreases from 400 (200) to 6 (1) ps for MAPb-I(3) (-Br(3)). By contrast, we found negligible temperature-dependent variations in τ for a mixed cation/mixed halide FA(0.85)MA(0.15)Pb(I(0.85)Br(0.15))(3). From temperature-dependent time-resolved microwave conductance measurements we conclude that the dipolar reorientation of the MA cation does not affect charge carrier mobility and lifetime in MHPs. Therefore, charge carriers do not feel the relatively slow-moving MA cations, despite their great impact on the dielectric constants.
format Online
Article
Text
id pubmed-6734799
institution National Center for Biotechnology Information
language English
publishDate 2019
publisher American Chemical Society
record_format MEDLINE/PubMed
spelling pubmed-67347992019-09-12 Charge Carriers Are Not Affected by the Relatively Slow-Rotating Methylammonium Cations in Lead Halide Perovskite Thin Films Caselli, Valentina M. Fischer, Mathias Meggiolaro, Daniele Mosconi, Edoardo De Angelis, Filippo Stranks, Samuel D. Baumann, Andreas Dyakonov, Vladimir Hutter, Eline M. Savenije, Tom J. J Phys Chem Lett [Image: see text] Recently, several studies have investigated dielectric properties as a possible origin of the exceptional optoelectronic properties of metal halide perovskites (MHPs). In this study we investigated the temperature-dependent dielectric behavior of different MHP films at different frequencies. In the gigahertz regime, dielectric losses in methylammonium-based samples are dominated by the rotational dynamics of the organic cation. Upon increasing the temperature from 160 to 300 K, the rotational relaxation time, τ, decreases from 400 (200) to 6 (1) ps for MAPb-I(3) (-Br(3)). By contrast, we found negligible temperature-dependent variations in τ for a mixed cation/mixed halide FA(0.85)MA(0.15)Pb(I(0.85)Br(0.15))(3). From temperature-dependent time-resolved microwave conductance measurements we conclude that the dipolar reorientation of the MA cation does not affect charge carrier mobility and lifetime in MHPs. Therefore, charge carriers do not feel the relatively slow-moving MA cations, despite their great impact on the dielectric constants. American Chemical Society 2019-08-09 2019-09-05 /pmc/articles/PMC6734799/ /pubmed/31398042 http://dx.doi.org/10.1021/acs.jpclett.9b02160 Text en Copyright © 2019 American Chemical Society This is an open access article published under a Creative Commons Non-Commercial No Derivative Works (CC-BY-NC-ND) Attribution License (http://pubs.acs.org/page/policy/authorchoice_ccbyncnd_termsofuse.html) , which permits copying and redistribution of the article, and creation of adaptations, all for non-commercial purposes.
spellingShingle Caselli, Valentina M.
Fischer, Mathias
Meggiolaro, Daniele
Mosconi, Edoardo
De Angelis, Filippo
Stranks, Samuel D.
Baumann, Andreas
Dyakonov, Vladimir
Hutter, Eline M.
Savenije, Tom J.
Charge Carriers Are Not Affected by the Relatively Slow-Rotating Methylammonium Cations in Lead Halide Perovskite Thin Films
title Charge Carriers Are Not Affected by the Relatively Slow-Rotating Methylammonium Cations in Lead Halide Perovskite Thin Films
title_full Charge Carriers Are Not Affected by the Relatively Slow-Rotating Methylammonium Cations in Lead Halide Perovskite Thin Films
title_fullStr Charge Carriers Are Not Affected by the Relatively Slow-Rotating Methylammonium Cations in Lead Halide Perovskite Thin Films
title_full_unstemmed Charge Carriers Are Not Affected by the Relatively Slow-Rotating Methylammonium Cations in Lead Halide Perovskite Thin Films
title_short Charge Carriers Are Not Affected by the Relatively Slow-Rotating Methylammonium Cations in Lead Halide Perovskite Thin Films
title_sort charge carriers are not affected by the relatively slow-rotating methylammonium cations in lead halide perovskite thin films
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6734799/
https://www.ncbi.nlm.nih.gov/pubmed/31398042
http://dx.doi.org/10.1021/acs.jpclett.9b02160
work_keys_str_mv AT casellivalentinam chargecarriersarenotaffectedbytherelativelyslowrotatingmethylammoniumcationsinleadhalideperovskitethinfilms
AT fischermathias chargecarriersarenotaffectedbytherelativelyslowrotatingmethylammoniumcationsinleadhalideperovskitethinfilms
AT meggiolarodaniele chargecarriersarenotaffectedbytherelativelyslowrotatingmethylammoniumcationsinleadhalideperovskitethinfilms
AT mosconiedoardo chargecarriersarenotaffectedbytherelativelyslowrotatingmethylammoniumcationsinleadhalideperovskitethinfilms
AT deangelisfilippo chargecarriersarenotaffectedbytherelativelyslowrotatingmethylammoniumcationsinleadhalideperovskitethinfilms
AT strankssamueld chargecarriersarenotaffectedbytherelativelyslowrotatingmethylammoniumcationsinleadhalideperovskitethinfilms
AT baumannandreas chargecarriersarenotaffectedbytherelativelyslowrotatingmethylammoniumcationsinleadhalideperovskitethinfilms
AT dyakonovvladimir chargecarriersarenotaffectedbytherelativelyslowrotatingmethylammoniumcationsinleadhalideperovskitethinfilms
AT hutterelinem chargecarriersarenotaffectedbytherelativelyslowrotatingmethylammoniumcationsinleadhalideperovskitethinfilms
AT savenijetomj chargecarriersarenotaffectedbytherelativelyslowrotatingmethylammoniumcationsinleadhalideperovskitethinfilms